Coherent Raman scattering with plasmonic antennas

Coherent Raman scattering (CRS) techniques are recognized for their ability to induce and detect vibrational coherences in molecular samples. The generation of coherent light fields in CRS produces much stronger signals than what is common in incoherent Raman spectroscopy, while also enabling direct views of evolving molecular vibrations. Despite the attractive attributes of CRS spectroscopy, the technique’s sensitivity is insufficient for performing measurements on single molecules, thus precluding the ability to coherently drive, manipulate and observe individual vibrational quantum oscillators with light. The single-molecule sensitivity that has been achieved in surface-enhanced Raman scattering (SERS) with the aid of plasmonic antennas suggests that a similar approach may be used to push CRS techniques to the single-molecule detection limit. Compared with SERS, however, experimental successes in surface-enhanced coherent Raman scattering (SE-CRS) are few, and a theoretical understanding of surface-enhancement in CRS is still incomplete. In this review, we discuss some of the principles and challenges in SE-CRS and summarize the latest advances in the quest of performing routine CRS experiments on single molecules.